CO₂ sequestration through mineral carbonation of iron oxyhydroxides.

Carbon dioxide sequestration via the use of sulfide reductants and mineral carbonation of the iron oxyhydroxide polymorphs lepidocrocite, goethite, and akaganeite with supercritical CO(2) (scCO(2)) was investigated using in situ attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), X-ray diffraction (XRD), and transmission electron microscopy (TEM). The exposure of the different iron oxyhydroxides to aqueous sulfide in contact with scCO(2) at ∼70-100 °C resulted in the partial transformation of the minerals to siderite (FeCO(3)) and sulfide phases such as pyrite (FeS(2)). The relative yield of siderite to iron sulfide bearing mineral product was a strong function of the initial sulfide concentration. The order of mineral reactivity with regard to the amount of siderite formation in the scCO(2)/sulfide environment for a specific reaction time was goethite < lepidocrocite ≤ akaganeite. Given the presence of goethite in sedimentary formations, this conversion reaction may have relevance to the subsurface sequestration and geologic storage of carbon dioxide.

[1]  C. Grey,et al.  Phosphate adsorption on the iron oxyhydroxides goethite (α-FeOOH), akaganeite (β-FeOOH), and lepidocrocite (γ-FeOOH): a 31P NMR Study , 2011 .

[2]  M. Schoonen,et al.  Hematite reactivity with supercritical CO2 and aqueous sulfide , 2011 .

[3]  P Renforth,et al.  Silicate production and availability for mineral carbonation. , 2011, Environmental science & technology.

[4]  Martin A. A. Schoonen,et al.  Ferrihydrite phase transformation in the presence of aqueous sulfide and supercritical CO2 , 2010 .

[5]  Stefan Bachu,et al.  CO2 storage in geological media: Role, means, status and barriers to deployment , 2008 .

[6]  A. Navrotsky,et al.  Size-Driven Structural and Thermodynamic Complexity in Iron Oxides , 2008, Science.

[7]  Yuhan Sun,et al.  Fe(II)-induced transformation from ferrihydrite to lepidocrocite and goethite , 2007 .

[8]  D. Postma,et al.  The reactivity of iron oxides towards reductive dissolution with ascorbic acid in a shallow sandy aquifer (Rømø, Denmark) , 2006 .

[9]  Robert J. Rosenbauer,et al.  Ferric iron in sediments as a novel CO2 mineral trap: CO2-SO2 reaction with hematite , 2005 .

[10]  Yousif K. Kharaka,et al.  Ferric iron-bearing sediments as a mineral trap for CO2 sequestration: Iron reduction using sulfur-bearing waste gas , 2005 .

[11]  Eric H. Oelkers,et al.  Geochemical aspects of CO2 sequestration , 2005 .

[12]  M. Krom,et al.  A revised scheme for the reactivity of iron (oxyhydr)oxide minerals towards dissolved sulfide , 2004 .

[13]  S. Poulton Sulfide oxidation and iron dissolution kinetics during the reaction of dissolved sulfide with ferrihydrite , 2003 .

[14]  A. Navrotsky,et al.  Thermodynamics of Fe oxides: Part I. Entropy at standard temperature and pressure and heat capacity of goethite (α-FeOOH), lepidocrocite (γ-FeOOH), and maghemite (γ-Fe2O3) , 2003 .

[15]  J. P. Labbe,et al.  Physico-chemical characterization of corrosion layers formed on iron in a sodium carbonate-bicarbonate containing environment , 1995 .

[16]  B. Wehrli,et al.  Kinetics and mechanism of the reaction of hydrogen sulfide with lepidocrocite , 1992 .

[17]  W. Stumm,et al.  Reductive dissolution of iron(III) (hydr)oxides by hydrogen sulfide , 1992 .

[18]  M. Schoonen,et al.  Reactions forming pyrite and marcasite from solution: I. Nucleation of FeS2 below 100°C , 1991 .

[19]  S. Warne,et al.  Examination of the siderite-magnesite mineral series by Fourier transform infrared spectroscopy , 1989 .

[20]  D. Bish,et al.  Quantitative phase analysis using the Rietveld method , 1988 .

[21]  R. J. Hill,et al.  Quantitative phase analysis from neutron powder diffraction data using the Rietveld method , 1987 .

[22]  S. Sommer,et al.  Sedimentary iron monosulfides: Kinetics and mechanism of formation , 1981 .

[23]  D. Rickard Kinetics and the mechanism of sulfidation of goethite , 1974 .

[24]  H. Rietveld A profile refinement method for nuclear and magnetic structures , 1969 .

[25]  C.A.J. Appelo,et al.  User's guide to PHREEQC - a computer program for speciation,batch-reaction, one-dimensional transport, and inversegeochemical calculations. , 1999 .

[26]  D. L. Parkhurst,et al.  User's guide to PHREEQC (Version 2)-a computer program for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations , 1999 .